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Transcript of 10.Wiegand, 2007
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344 d e n t a l m a t e r i a l s 2 3 ( 2 0 0 7 ) 343362
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 344
2. Fluoride release of restorative materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 344
2.1. Glass-ionomer cements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 344
2.2. Resin-modified glass-ionomer cements and polyacid-modified composites . . .. .. . .. .. .. . .. .. . .. .. .. . .. .. . .. .. .. . 345
2.3. Composite . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 346
2.4. Amalgam . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 347
3. Factors influencing the release of fluoride from restoratives. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. .. . 347
4. Fluoride recharge of restorative materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 348
5. Clinical relevance of fluoride released from restoratives in human saliva and plaque. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 349
6. Antimicrobial activity of fluoride-releasing materials . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 349
7. Fluoride uptake of adjacent tooth structure . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 350
8. Influence of fluoride-releasing restoratives on caries development and progression . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 351
8.1. Influence on demineralization of enamel adjacent to fluoride-releasing restoratives . . . . . . . . . . . . . . . . . . . . . . . . . . . . 351
8.1.1. In vitro studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 351
8.1.2. In situ and in vivo studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 352
8.2. Influence on demineralization of dentin adjacent to fluoride-releasing restoratives . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 353
8.2.1. In vitro studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 353
8.2.2. In situ studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 353
8.3. Clinical studies evaluating secondary caries adjacent to fluoride-releasing restoratives . . . . . . . . . . . . . . . . . . . . . . . . . 353
9. Influence on caries formation of teeth located in interproximal contact to fluoride-releasing restoratives . . . . . . . . . . . . 354
9.1. In vitro and in situ studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 354
9.2. Clinical studies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 354
10. Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 355
Acknowledgement . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 355
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 355
1. Introduction
Since the observation that secondary caries formation wasrarely associated with fluoride-containing silicate cement
restorations, increasing attention has been focused on the
development of various fluoride-releasing products, to be
used as restorative materials, lining cements, sealants and
orthodontic cements.
Fluoride is well documented as an anticariogenic agent.
A variety of mechanisms are involved in the anticariogenic
effects of fluoride, including the reduction of demineraliza-
tion, the enhancement of remineralization, the interference of
pellicle and plaque formation and the inhibition of microbial
growth and metabolism [14]. Fluoride released from dental
restorative materials is assumed to affect caries formation
through all these mechanisms and may therefore reduce orprevent demineralization and promote remineralization of
dental hard tissues.
Today, there are several fluoride-containing dental restora-
tives available in the market including glass-ionomers, resin-
modified glass-ionomer cements, polyacid-modified com-
posites (compomers), composites and amalgams. Due to
their different matrices and setting mechanisms the prod-
ucts vary in their ability to release fluoride. However, it is
assumed that the antibacterial and cariostatic properties of
restoratives are often associated with the amount of fluoride
released.
This paper aimed to summarize the current status of
fluoride-releasing dental restoratives, their ability to release
and recharge fluoride, their antibacterial activity and car-
iostatic properties. Therefore, original scientific papers and
reviews listed in PubMed or available from peer-reviewed Ger-
manjournals (publishedbetween 1980 and 2004) were includedin the review. Clinical studies concerning the development of
secondary caries at the margin of restorations were taken into
consideration when performed in split-mouth design with an
observation period of at least three years. Papers dealing with
orthodontic or endodontic topics were not included in the
review.
2. Fluoride release of restorative materials
2.1. Glass-ionomer cements
Glass-ionomer cements are composed of fluoride-containing
silicate glass and polyalkenoic acids which are set by anacidbase reaction between the components. During the set-
ting reaction a variety of ionic constituents is released from
the glass, including fluoride. Two mechanisms have been pro-
posed by which fluoride may be released from glass-ionomers
intoan aqueous environment. One mechanism is a short-term
reaction, which involves rapid dissolution from outer surface
into solution (process I), whereas the second is more gradual
and resulted in the sustained diffusion of ions through the
bulk cement (process II) [59]. These processes are presented
by the right-hand first and second terms of the equation:
[F]c = [F]It/(t + t1/2)+ t. The parameter t1/2 is the so-called
half-life of the process I to reach one-half of its maximum
value which is given by F. Parameter t is material depen-
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dent and can be considered as a measure for the driving force
of process II. Forthe mostconventional and the resin-modified
glass-ionomers and some high fluoride-releasing compomers
and composites, the process follows a square root depency
on time suggesting that in some way a concentration gradi-
ent would be responsible for the driving force of the elution
[5,10].
An initial high release from glass-ionomers over the first24h is likelydue to theburst of fluoride released from theglass
particles whenreacting withthe polyalkenoateacid during the
setting reaction.
Karantakis et al. [11] evaluatedthat the highest fluoride dis-
solution occurred especially during the first 4 h after mixing
amounting to 1.61.8g/mm2. Bell et al. [12] showed that the
concentration of fluoride releasedfrom glass-ionomer cement
specimens (1.5mm thick, 6 mm in diameter) into artificial
saliva within 10min after immersion amounted to 1 ppm and
that the cumulative total fluoride in the first 24 h was nearly
15 ppm. In vitro, it is frequently confirmed that the maxi-
mum release occurred during the first 2448 h [1218] rang-
ing from 5 to 155 ppm for different brands of glass-ionomercements (11.5mm thick, 6mm in diameter) [12,14,1619].
Metal-reinforced glass-ionomers seem to release less fluo-
ride than conventional glass-ionomer cements [8,2026]. This
effect may be explainedby the initial lower fluoride content of
these materials due to the replacement by silver or the forma-
tion of silver fluoride which binds the fluoride ions into the
cement preventing leaching of the fluoride [21]. In contrast,
in glass-ionomers containing bioactive glass [27] or casein
phosphopeptideamorphous calcium phosphate [28] fluoride
release seems to be increased comparedto conventionalglass-
ionomers.
After the initial burst, fluoride release slows down and
is followed by a prolonged long-term fluoride release, whichoccurs when the glass dissolves in the acidified water of
the hydrogel matrix [22,29]. Studies have shown that the
cumulative amount of fluoride ions released from glass-
ionomer cements, after a short period of time, is diffusion
controlled and follows a decreasing gradient, which is lin-
ear to the square root of time [10,3032]. Thereby, the ini-
tial high amounts of fluoride rapidly decrease after 2472 h
[11,26,33] and plateaued to a nearly constantlevel within 1020
days [8,15,26,29,34]. After 510 days the cumulative amount
of leached fluoride is about 0.33g/mm2 [11,29,35]. Creanor
et al. [14] found that the concentration of leached fluoride
in deionized water had slowed from 15155 ppm at day 1 to
about 0.94ppm at day 60. After one year, the steady statefluoride release of four different glass-ionomers was approx-
imately 0.57ppm as shown by Perrin et al. [36]. In other in
vitro studies, long-term fluoride release from glass-ionomers
is reported to occur from several months to over three years
[8,14,23,37,38].
In vivo, fluoride concentration of unstimulated saliva
measured immediately after placement of one to six glass-
ionomer restorations increased from approximately 0.04 to
0.81.2 ppm. However, after three weeks the fluoride release
diminished by about 35% and after six weeks for an additional
30% [39]. Nevertheless, the fluoride level in saliva after one
year amounted to 0.3 ppm and was therefore 10 times higher
as baseline values [40].
2.2. Resin-modified glass-ionomer cements and
polyacid-modified composites
Resin-modified glass-ionomer and polyacid-modified com-
posite restoratives have been developed to overcome the
problems of moisture sensitivity and low initial mechanical
strengths typical for conventional glass-ionomers. Polyacid-
modified resin composites (compomers) claim to combine themechanical and esthetic properties of composites with the
fluoride-releasing advantages of conventional glass-ionomer
cements.
Resin-modified glass-ionomers were basically formed
by adding methacrylate components to the polyacrylic
acid, which are polymerizable by light-curing supplement-
ing the fundamental acidbase reaction. Polyacid-modified
resin composites consist of conventional macromonomers
also used in composites, such as Bisphenol-Glycidyl-
dimethacrylate or urethane dimethacrylate, together with
small amounts of acid-functional monomers. The filler glass
is identical to the ion-leachable glass fillers used in conven-
tional glass-ionomer cements but in smaller sizes as knownfromcomposites.Initial setting is performed by light-activated
polymerization which is followed by an acidbase reaction
that arises from sorption of water. Recently, a new category
of hybrid material (giomers) was introduced in the interna-
tional market. Giomers include pre-reacted glass-ionomers to
form a stable phase of glass-ionomer fillers in the restora-
tive. Unlike compomers, fluoro-alumino-silicate glass parti-
cles react with polyacrylic acid prior to inclusion into theresin
matrix.
Resin-modified glass-ionomers were mostly found to have
a potential for releasing fluoride in equivalent amountsas con-
ventional cements [41], but may be affected not only by the
formation of complex fluoride compounds and their interac-tion with polyacrylic acid, but also by the type and amount
of resin used for the photochemical polymerization reaction
[4244]. The kinetics of the cumulative fluoride release of
most resin-modified glass-ionomers are summarized by Ver-
beeck et al. [5] and Xu and Burgess [10] as described above:
[F]c = [F]It/(t + t1/2)+ t.
Fluoride release from different resin-modified glass-
ionomer cements is also highest during the first 24h and
amounted to 535g/cm2 depending on the storage media
[11,15,16,35,45,46]. Mean concentration of fluoride release
from resin-modified glass-ionomer specimens (1.5 mm thick,
6 mm in diameter) into deionizedwater over thefirst 24 h after
setting amounted from 2265ppm for the first 6 h to 320 ppmfor the 1824h period [14]. Daily release rates dropped from
815 ppm (1st day) to 12 ppm (7th day) within 1 week [16,17]
and are stabilized from 10 days [14,33] to 3 weeks [47]. Resin-
modified glass-ionomers continue to release fluoride in small
amountsin vitro (about 12ppm, depending on the specimens
size) for 12.7 years [8,11,37,45,46,48,49].
In contrast to the conventional and resin-modified glass-
ionomers, polyacid-modified composites are mostly shown to
have no initial fluoride burst effect [16,17,48,50], but levels of
fluoride release remain relatively constant over time [17,51].
For the most polyacid-modified composite resins and micro-
filled composite resins, the zero-order kinetics are indicative
of a matrix-controlled elution: [F]c = [F]It/(t + t1/2) +t. Thereby,
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346 d e n t a l m a t e r i a l s 2 3 ( 2 0 0 7 ) 343362
values of are material dependent and can be considered as
measure for the driving force of this process [5,10].
However, short-term fluoride release is slightly increased
during the first few days [17,35,52], but is quite clearly lower
compared to conventional or resin-modified glass-ionomers
[18,33,48,51,5356]. However, thisfinding was not corroborated
by a study ofAttinet al. [57] who found higher fluoride release
for compomers than for glass-ionomer cements. The authorsexplained these differences by the composition of the com-
pomer brands, which exhibited a higher fluoride content and
contained smaller fillers, which might lead to a better reactiv-
ity due to the greater size of the specific surface.
However, the difference between glass-ionomers and
polyacid-modified resin composites during the first phase of
fluoride release could be due to the fact that after curing and
before contact with water the fluoride in polyacid-modified
composites is not free but bound in the filler particles which
are enclosedin thepolymerized matrix. It should be notedthat
in the first phaseof setting, whichis a light-activatedpolymer-
ization, polyacid-modified composites completely behave like
composites. Also, in the second process of fluoride release,dif-fusion of fluoride in a period of up to six months was reported
to be smaller in polyacid-modified resin composites and com-
posites than in glass-ionomers [11,29]. This mechanism is
discussed to be the result from a more tightly bound and/or
less hydrophilic matrix of the composite resin [29]. However,
Asmussen and Peutzfeld [38] found that compomers might
release relatively little fluoride during the first year after set-
ting, but after this time the rate of fluoride release became
equal to that of glass-ionomers.
The main filler fraction in compomers and composites
does differ significantly. When in composites rather inert Ba-
glasses or alike are typically used, the filler glass in a typical
compomer is identical to that of glass-ionomers. Additionallystrontium fluoride or ytterbium trifluoride is added for radio
opacity and may increase fluoride release, too.
With regard to compomers, several authors found differ-
ences in fluoride release in products with different filler sys-
tems. Compomers containing glass fillers and ytterbiumtriflu-
oride are reported to release higher amounts of fluoride than
SrF2-containing products [18,5763].
Daily fluoride release into an aqueous solution from com-
pomers (1.5 mm thick, 6 mm in diameter) declines from
12.4 ppm for the 1st day to 0.170.23ppm after 60 days [18].
With time the initially light cured material takes up water,
and the carboxylic groups of the acidic monomer promote an
acid/base reaction with metal ions of the glass filler. The sub-sequent water sorption leads to ionization of the acid groups.
This reaction takes place at a slow rate and reaches a satu-
ration point after approximately four weeks [64]. Due to this
kinetics, cumulative fluoride release of compomersduring the
first days is expected to be low as compared to conventional
glass-ionomers [17].
Cumulative fluoride release from compomers into deion-
ized water amounted to 0.080.12g/mm2 after 7 days and to
0.390.41g/mm2 after 91 days [29]. After 253 days, weekly flu-
oride release into deionizedwater was reportedto be 0.76 ppm
or rather 1.92g/cm2 [48]. Long-term release of fluoride from
compomers was followed and measured up to three years
[38,48].
Currently, less information is available about fluoride
released from giomers [17,65]. Also, for giomers, no ini-
tial burst effect could be observed. Amounts of fluoride
leached from giomers seem to be slightly higher than from
composites and compomers but lower compared to glass-
ionomers [17,65]. After 24 h, mean fluoride release from spec-
imens (1 mm thick, 6 mm in diameter) into deionized water
amountedto 4.54 ppm anddropped to 0.06 ppm perday withinone week [17].
2.3. Composite
Resin composites may contain fluoride in a variety of forms,
such as inorganic salts, leachable glasses or organic fluoride.
Thereby, not only the amount of fluoride but type and particle
size of the fluoridated filler, the type of resin, silane treat-
ment and porosity might be important factors contributing
to fluoride release [10,6669]. Moreover, the fluoride release
increased with the hydrophilicity and the acid character of
the polymer matrix [38].
Three different approaches for the development offluoride-releasing composites have been reported including
the addition of water-soluble salts such as NaF or SnF2,
fluoride-releasing filler systems or matrix bound fluoride (for
review see [67]).
Incorporation of inorganic fluoride has resulted in
increased fluoride release, but leads to voids in the matrix as
the fluoride leaches out of the material. Dispersion of leach-
able glass or soluble fluoride salts into the polymer matrix
allows for a water-soluble diffusion of fluoride from the com-
posite resin in the local environment. Most of the fluoride
is already released during the setting reaction, followed by a
smaller amount of long-term fluoride release.
Mainly twofillertypes can be distinguished, sparingly solu-ble compounds, such as strontium fluoride (SrF2) or ytterbium
trifluoride (YbF3) and leachable glass fillers [10,59,67]. The
composites in which the radioopaque fluoridated filler YbF3was used most likely release fluoride by means of an exchange
reaction. Water diffusion into the composite causes fluoride
release from the particles followed by a diffusion gradient
driven movement into the environmental solution (water and
saliva). As mentioned before, fluoride silicate fillers in glass-
ionomers and resin-modified glass-ionomersare moresoluble
and thus release more fluoride especially when reacting with
the polyacrylic acid. Finally, organic fluoride components have
been added to the matrix to increase the fluoride release.
Matrix bound fluoridesare available such as acrylic-amine-HF-salts, methacryloyl acid-fluoride and acrylic-amine-BF3 [70].
Fluoride levels leached from composites are mostly much
lower compared to levels released from conventional or resin-
modified glass-ionomers and also somewhat lower as com-
pared to polyacid-modified composites [11,18,29,37,38,71,72].
Initial fluoride release into deionized water within 24h
amounted to 0.042.7ppm for different composite brands
(1.5 mm thick, 6 mm in diameter), but decreased to 0.022ppm
within 3060 days [16,18]. Weekly release from specimens
(1 mm thick, 15 mm in diameter) is also reported to decrease
from 34 to 12ppm within a few weeks [73]. Cumulative
fluoride-releasing rates in artificial saliva, lactic acid or deion-
ized water amounted to less than 0.5 g/mm2 during 90120
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d e n t a l m a t e r i a l s 2 3 ( 2 0 0 7 ) 343362 347
days [11,29]. Long-term release of different commercial and
experimental resin composites is reported to last for up to five
years [66,7476].
It could be shown that experimental highly fluori-
dated composites and an ion-releasing composite (Ariston)
released higher amounts of fluoride than conventional flu-
oridated composites [16,66,77]. While most commercially
available composites exhibited a fluoride release which isapproximately proportional to the logarithm of time or to
t1/2 [66,73], an experimental high-fluoridated compositeshowed a linear fluoride release, which is proportional to t
[66,78].
The high fluoride release of these experimental or high-
fluoridated composites is discussed to be a result of a high
fluoride content (F-Al-silicate and YbF3) combined with high
watersolubilityof the filler, high water uptake anda highly dif-
fusible polymer matrix [10,16,66], the latter two reasons being
the cause for clinical failures as shown by Braun et al. [79] and
Merte et al. [80].
2.4. Amalgam
Several studies investigated fluoride levels released from
amalgam [23,8184]. Storage of conventional amalgam class
V restorations in deionized water revealed fluoride values
of less than 0.02 ppm within four weeks [84] and less than
0.08ppm one year after insertion [83]. Cumulative fluoride
content after placement of amalgam specimens (1.6 mm
thick, 15.2mm in diameter) in artificial saliva amounted to
less than 0.1g/mm2 within seven weeks [82]. These results
are also confirmed for fluoride-containing amalgam samples
(2mm2 mm12mm) [85]. The initial release of fluoride intohydroxyapatite decreased from 0.33 to 0.009g/mg withinone
week [85].In summary, fluoride release from different fluoridated
restorative materials may last for a long period. However, after
a higher initial release, fluoride release from these materials
may drop to very low levels.
3. Factors influencing the release offluoride from restoratives
The elution of fluoride is a complex process. It can be affected
by several intrinsic variables, such as formulation and fillers
[27,28,31,42,86,87]. It is also influenced by experimental fac-
tors, i.e. storage media, frequency of change of the storagesolution, composition and pH-value of saliva, plaque and
pellicle formation [9,12,21,32,35,52,8894]. It was shown that
the powderliquid ratio of two-phase-systems, mixing proce-
dure, curing time and the amount of exposed area as well
as the different storage media affected the fluoride release
[21,29,32,36,92,9598]. In vitro, fluoride release was dependent
on exposed surface area and not on sample weight [32]. Radi-
antheat applied to glass-ionomers at different intensities and
for different time intervals using a high-intensity fibreoptic
quartz tungsten halogen light source had no effect of fluoride
release [99].
Several laboratory studies investigated the quantity of
fluoride released into water, artificial saliva or acidic solu-
tions. Kinetic findings demonstrated that the patterns of flu-
oride release from conventional and resin-modified glass-
ionomers as well as compomeres and composites in dif-
ferent storage media were similar. However, the amount of
daily and accumulated fluoride release of these materials
is different as mentioned above [11]. On long term, com-
posites have mostly shown to release lower amounts of
fluoride compared to glass-ionomer, resin modified glass-ionomer and compomer [11,23,29,38]. In general, the highest
release is found in acidic and demineralizingremineralizing
regimes andthe lowest in saliva [11,35,52,53,57,71,94,100102].
Demineralizingremineralizing regimes are chosen for sim-
ulating the pH-cycling that occurs during caries attack. The
increasing amount of fluoride in acidic media could be
explained by the fact that a decrease in pH increases the dis-
solution of the material leading to a higher fluoride level in
the acidic immersion [11,52,63,94,102,103]. Thereby, the pro-
portion of free (uncomplexed) fluoride to bound (complexed)
fluoride was lower under acidic than under neutral condi-
tions [94,103]. Artificial saliva tends to decrease the amount
of leached fluoride to 1725% of that found in water [12]. Thisobservation might be explained by the fact that the diffusion
gradient between the restorative material and ion-enriched
saliva is lower as compared to the gradient between the
restorative and distilled water. Moreover, it is suggested that
components from saliva form a pellicle on the surface of the
restorative material that impedes ion release [8,12,101,104].
Bell et al. [12] showed that salivary depositson glass-ionomers
formed within the first 10 min after immersion into saliva
caused a retarding effect on fluoride release. Moreover, Arends
et al. [67] found that the presence of a pellicle reduced the
fluoride-releasing rate of a fluoridated composite by about
1520%.
Nevertheless, in human saliva fluoride rates may beincreased due to the activity of salivary enzymes. It was
demonstrated that fluoride release from resin-modified glass-
ionomers and compomers may be increased in esterase-
containing artificial saliva compared to artificial saliva free
of enzymes [105107]. It was also discussed that plaque-
associated organic acids or salivary hydrolases may increase
initial fluoride release in vivo [107]. The clinical relevance of
fluoride released in human saliva or plaque will be discussed
separately.
It should be noted that covering of the materials with
adhesives or bonding agents may influence the short- and
long-term release of components of dental filling materials.
Immediateapplicationof a surface coating agent might alsobeperformed to protect glass-ionomers from moisture contam-
ination and dehydration during initial setting. Even though
fluoride-containing dental adhesives are able to release flu-
oride in a range from 4 to 30 g/cm2 during eight weeks
[46,108,109], adhesive coating of the material surface signif-
icantly reduces the amount of fluoride leached from glass-
ionomers and compomers [15,62,90,100,110,111]. In vitro, flu-
oride leached from filling materials coated with an adhesive
was reduced by a factor 1.54 [62,112,113].
Neither bleaching nor brushing of restorative materials
increased the amount of fluoride release. Home-bleaching or
in-office bleaching agents containing 10 or 35% carbamide
peroxide have shown to be ineffective in increasing the
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release of fluoride from conventional and resin-modified
glass-ionomers as well as composites [114].
Removal of the outermost layer of compomers by air-
polishing or finishing maylead to an increased fluoride release
[90,115]. This pattern was explained by the fact that air-
polishing removes the outer surface of a water-immersed
specimen which leads to exposition of deeper zones of the
material not depleted of fluoride. However, simulation of oralhygiene behavior by brushing of a polyacid-modified compos-
ite with a fluoride-free dentifrice didnot maintain the initially
high level of fluoride release for a longer period of time com-
pared to unbrushed samples [60].
4. Fluoride recharge of restorative materials
The cariostatic action associated with fluoride-releasing
materials is usually attributed to a sustained release of fluo-
ride. Due to the fact that fluoride levels leached from fluoride-
containing filling materials decreased over time (which is
significant for glass-ionomers and resin modified glass-ionomers), the recharging of restoratives with fluoride has
been suggested to maintain a continuously increased level of
fluoride release. The ability of a restorative to act as a fluoride
reservoir is mainly dependent on the type and permeability of
filling material, on the frequency of fluoride exposure and on
the kind and concentration of the fluoridating agent [116,117].
A review of previous in vitro and in situ studies showed that
various methods of aging (deionized water, distilled water and
artificial/human saliva), periods of aging (days to months) and
methods of fluoride recharge may also actas contributory fac-
tors [52,117122].
Fluoride release after application of fluoridated agents may
occur partly by washout of fluoride ions that are retained onthe surface or inthe poresof therestorative. Surface boundflu-
oride might be more easily detached during an acidic attack,
such as erosions. Also, free fluoride incorporated into the
matrix might be washed out [47].
Glass-ionomers are mostly found to have significantly bet-
ter capability to act as a fluoride reservoir than composite
resin-based materials [18,52,72,77]. This fact can be explained
by the loosely bound water and the solutes in the porosi-
ties in the glass-ionomer, which may be exchanged with an
external medium by passive diffusion [10,123]. The absorp-
tion and re-release of fluoride might be determined by the
permeability of the material. Thus, a completely permeable
substance could absorb the ions deep into its bulk, while arelatively impermeable material can only absorb fluoride into
the immediate subsurface [116]. Therefore, the slight increase
of fluoride release from resin-based restoratives after expo-
sure to exogenous fluoride is discussed to be most probably
because of surface-retained fluoride [18]. In general, materi-
als with higher initial fluoride release have higher recharge
capability [10,16,124,125]. However, fluoride release from aged
and refluoridated specimens mostly did not reach the initial
fluoride release of the material [16,18,126].
In vitro, comparison of fluoride leached from one-
time refluoridated conventional and resin-modified glass-
ionomers, ion-releasing composite as well as flowable
and packable compomers and composites showed an
increased fluoride release for 24 h followed by a rapid return
to near pre-exposure levels already within several days
[16,18,120,126128]. Three months after single application of
1.23% APF to aged restorative materials, fluoride release of
glass-ionomers and compomers was even lower than imme-
diately before gel application [125].
Refluoridation of glass-ionomers, compomers and com-
posites with a 500 ppm F solution 13 times over a two-yearperiod revealed different capacities among the materials with
respect to absorbtion and release of fluoride. After 720 days,
glass-ionomer-based materials displayed a far better poten-
tial to re-release fluoride (312gF/cm2, 1 h post-recharge)
than composites (0.20.3gF/cm2, 1 h post-recharge) and per-
formed somewhat better than compomers (3.65gF/cm2, 1 h
post-recharge) [72].
In the oral environment, dental restorations are frequently
exposed to exogenous sources of fluoride, such as fluori-
dated dentifrices, and mouth rinses or high-dose fluoride gels
and varnishes. Regular fluoridation of restorative materials
is mainly performed by toothbrushing with fluoridated den-
tifrices or fluoride gels.Daily exposition of filling materials to fluoridated den-
tifrices has demonstrated a high rechargibility for glass-
ionomers [52,119,122,129], while the replenishment of resin-
based materialsseemsto be negligibly small [52,77,122]. Olsen
etal. [129] evaluated fluoride release of an aged resin-modified
glass-ionomer after daily exposure (30 min daily over 10 days)
to different toothpaste slurries. Application of fluoridated
(0.05%) and non-fluoridated dentifrices with pH 2.5, 5.7 and
8.3 increased the amount of fluoride release during the expo-
sure period, but was highest for the acidic slurry regardless
whether it was fluoridated or not. However, after the expo-
sure period fluoride levels in all groups, except the fluori-
dated and non-fluoridated dentifrices with pH 2.5, decreasedbelow baseline rates within 10 days [129]. Moreover, a constant
decrease of fluoride release is also reported during the period
of daily toothpaste exposure [52,118]. Attin et al. [52] found
that 5 min toothpaste slurry (1250ppm F and 5ml artificialsaliva) application also increases the fluoride re-release from
glass-ionomer specimens but not from compomers. Fluoride
re-release of glass-ionomers might also be increased when
application of the fluoridated dentifrice is performedby brush-
ing of samples instead of storage of the samples in dentifrice
slurries only [130].
In general, refluoridation seems to be more effective with
increasing concentration of the agent [117,131] and frequency
of application [122,128] as well as under acidic conditionsof the environment [52,118], e.g. in a simulated high caries
challenge situation. This was also shown for fluoridation of
restoratives with fluoride gels and solutions [19]. Daily immer-
sion in 250, 1000 and 2500ppm fluoride solution increased
the amount of leached fluoride from glass-ionomers from 1
to 215 ppm per day over the experimental period [19]. Refluo-
ridation of compomers and conventional and resin-modified
glass-ionomers was also more effective after application of
0.2% NaF solution than after treatment with 0.02 or 0.04% NaF
solution [33,132], but fluoride levels did not exceed 6.5 ppm
[33]. With regard to the kind of fluoride, 1.23% APF gels seem
to be more effective than neutral 1% NaF gel and 0.001%
CaF2 or 4% SnF2 agents [47,133,134]. After refluoridation with
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phatase, peroxidase and catalase may be affected by fluoride
ions [154].
Although even low fluoride levels may reduce bacterial
growth, dental plaque composition and acid production in
vitro [156160], the clinical importance of the affection of
plaque metabolism by fluorides is still unclear [161,162]. Fluo-
ride concentrations needed for antimicrobial effects mostly
surpass the concentration needed to reduce the solubilityof apatite. In vitro, only small amounts of fluoride (approxi-
mately 0.030.08 ppm) in remineralizing solutions are neces-
sary to shift the equilibrium from demineralization to rem-
ineralization. Therefore, it is often considered that the antimi-
crobial effect of fluoride is less important when the fluoride
concentration required for inhibition of demineralization is
exceeded.
However, several clinical studies found that the fluoride
concentration of plaque on or adjacent to glass-ionomers
is increased and the proportion of mutans streptococci in
plaque is reduced [149,151,152,163165]. Fluoride levels of 14-
day-old plaque grown adjacent to glass-ionomers decreased
from 19,985ppm after 14 days to 5788ppm after 28 daysand 5019 ppm after 43 days, but was considerably higher
than fluoride concentration of plaque grown on composite
(about 200 ppm) [149]. Contradictory, Seppa et al. [148] found
no increased fluoride concentration of approximal plaque of
teeth close to glass-ionomer restorations either after two or
four weeks. In patients using fluoridated toothpastes, fluo-
ride levels detected in plaque adjacent to one-year-old resin-
modified glass-ionomer (6 nmol/mg), compomer (3 nmol/mg)
and resin composite (3.1nmol/mg) restorations were only
slightly increased compared to the fluoride content of enamel
plaque (1.2 nmol/mg) [166].
Even refluoridation of three-year-old glass-ionomers with
1.2% fluoride gel did not increase plaque fluoride concentra-tion significantly [149].
However, in a chemo-stat experiment it was shown that
fluoride can inhibit the growth of oral streptococci in vitro at
concentrations in the order of 0.160.31 mol/l [167]. This con-
centration is much higher as found in dental plaque adjacent
to fluorid-containing restoratives. Due to this fact, the results
of some in vivo investigations mostlyshowed that thefluoride
concentrations released from one- to three-year-old restora-
tives are not high enough to affect the metabolism of caries-
associated bacteria, e.g. mutans streptococci and lactobacilli
in dental plaque [150,166,168]. In contrast, studies investigat-
ing glass-ionomer restorationsup to one month after insertion
showed a correlation between fluoride release and reducedmutans streptococci counts in plaque [150,151,163165] or
saliva [39]. However, levels of mutans streptococci in plaque
from compositeor amalgam fillings were lower than in plaque
formed on glass-ionomers [150,163165].
The caries-preventive effect of resin-modified glass-
ionomers has also been related to decrease in microbial col-
onization of carious dentin. In vivo, a resin-modified glass-
ionomer restoration leads to a larger decrease in counts of
mutans streptococci and lactobacilli in remaining carious
dentin than amalgam [169,170]. In contrast, Weerheijm et al.
[171] found no differences in numbers of oral streptocci and
lactobacilliin dentinlesion two yearsafterinsertion of a glass-
ionomer or a resin-based sealant.
It has already been discussed that other components
simultaneously released from ionomeric-based (e.g. alu-
minium and zinc) or resin-based materials (monomers and
catalysts) may be involved in the antibacterial activity of the
materials [35,152,172].
In conclusion, fluoride is known to inhibit the biosyn-
thetic metabolism of bacteria, but these antimicrobial effects
in caries prevention are often regarded as little or of noimportance as compared to the direct interactions of fluo-
ride with the hard tissue during caries development and pro-
gression. There is still a lack in studies whether the antibac-
terial effects clinically contribute to the anticaries effect
of fluoride and whether fluoride leached from restoratives
into plaque or saliva may be relevant for these antibacterial
effects.
7. Fluoride uptake of adjacent toothstructure
For many years the cariostatic effect of fluoride was attributedto the incorporation of structurally bound fluoride in the
hydroxyapatite crystal lattice and the reduced solubility of the
so-formed fluoridated hydroxyapatite. However, recent obser-
vations have found that fluoride in the aqueous phase sur-
rounding the carbonated apatite crystals is much more effec-
tive in inhibiting demineralization than fluoride incorporated
into the crystals [4]. Fluoride may precipitate onto tooth sur-
faces as calcium fluoride-like layer, which serves as a reservoir
for fluoride when the pH drops [4]. This calcium fluoride-like
material, so-called KOH-soluble fluoride, facilitates the repre-
cipitation of minerals by forming fluoroapatite or fluorohy-
droxyapatite, thereby preventing further loss of mineral ions
[4,173]. Nevertheless, enamel resistance to lesion formationalso increased with increasing content of tooth-bound fluo-
ride [174].
Glass-ionomers and other fluoride-releasing restoratives
are reported to increase both the structurally bound and KOH-
soluble fluoride content of the adjacent dental hard tissues
[151,175182]. Fluoride uptake into dental hard tissues in the
absence of an acidic medium mainly occurs by slow diffu-
sion processes. Moreover, glass-ionomerscontaining bioactive
glass are shown to induce precipitation of calcium fluoride-
like compounds on dentin slabs, when immersed into simu-
lated body fluid [27].
Kawai et al. [175] investigated the amount of structurally
bound and KOH-soluble fluoride after fixation of fluoride-containing composite slabs onto enamel surfaces. Mean total
fluoride uptake at 10m depth amounted to 300600ppm and
decreased to approximately 200ppm at 30m depth. However,
amount of structurally bound and KOH-soluble fluoride at 10,
20and 30m depths was notsignificantly differentamongthe
different fluoridated composites [175]. In vivo, fluoride uptake
fromfluoridated composite slabs fixedto enamel surfacesalso
decreased only slightly from 785 to 590 ppm at levels from 2.5
to 50m depth [183].
The mean penetration depth of fluoride released from flu-
oridated composites into the enamel and dentin side walls of
class V restorations four weeks after insertion ranged from
19 to 47m [178]. Fluoride concentration at these cavity walls
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amounted to 42009400 ppm [178] which reflects the distinct
fluoride uptake.
For conventional and resin-modified glass-ionomers, flu-
oride uptake was also found to be highly significant in both
primary and permanent enamel [151,184]. Conventional glass-
ionomer cements seemed to be more effectively increasing
the content of fluoride in enamel and root surfaces than
metal-reinforced glass-ionomers due to a higher release offluoride [24,185]. In vitro, one month after application of glass-
ionomer-based restorations enamel fluoride uptake adjacent
to the restoration amounted to 24004100 ppm [181] and was
nearly the same after three and six months. In a distance of
1.57.5 mm to the margin of the restoration fluoride uptake by
more than 2000ppm was found [181].
Under in situ simulation of a high cariogenic challenge,
enamel fluoride uptake around glass-ionomers was twice
greater and mineral loss twice lower than in enamel restored
with non-fluoridating composites [151].
Enamel fluoride uptake in the vicinity of 1 or 5% SnF2silver amalgam restoration was found to be approximately
100200ppm after one month [182].Due to differences in microstructure and porosities of den-
tal hard tissues, the amount of fluoride uptake from restora-
tives and the depth of fluoride penetration are higher for both
dentin and cementum than for enamel [109,175,177,181,182].
Fluoride penetration fromdifferent restoratives intodentin
was highest for conventional glass-ionomers (300m, one
week after insertion) followed by resin-modified glass-
ionomers and composites [180]. Fluoride concentration of
dentin beneath a glass-ionomer cement filling might increase
to approximately 2000 ppm compared to the fluoride concen-
tration beneath a zinc phosphate cement filling [186]. Other
investigations found higher amounts of fluoride uptake for
fluoride-releasing resins (300012,000 ppm) [177,178] than forglass-ionomers (50006000 ppm) into side and axial walls of
dentin cavities [177]. One month after insertion of a glass-
ionomer restoration fluoride acquisition by cementumlocated
1.57.5 mm distant to the filling was about 14,00016,000ppm.
Reevaluation of fluoride uptake after three and six months
still revealed 60007000 and 50006000ppm, respectively [181].
After insertion of various fluoride-containing composites, the
concentration of total fluoride in cementum amounted to
2003500ppm at 10m depth and decreased to 1002500ppm
at 30m. Thereby, levels of bound fluoride uptake were
approximately 1002000ppm at 10m depth and501000ppm
at 30m depth [175].
An increase of fluoride concentrationin dental hard tissuesis also reportedfor SnF2 silver amalgam. Thereby, fluoride was
taken up to a greater extent from 5% SnF 2 than from 1% SnF2and was generally higher in dentin than in enamel [182].
As mentioned above, fluoride uptake from fluoride-
releasing restorations is higher in dentin and cementum than
in enamel, but is influenced by the interface between restora-
tion and tooth [180]. The presence of an intermediary micro-
gap or material layer between the restoration and the dental
hard tissues could restrict or promote the passage of fluoride.
Gapformation between the filling material and the cavity wall
will lead to a fluoride transport acrossthe fluid-filled gap. The-
oretically, a small gap withminimal fluidexchange will elevate
fluoride concentrationand create a greater diffusion potential.
Some of the fluoride will adsorb onto apatite crystallites and
become firmly bound. High concentrations of calcium, phos-
phate and fluoride at the interface may facilitate the precip-
itation of calcium fluoride-like compounds [187]. An infrared
spectroscopic analysis concluded that the interface between
glass-ionomers and dentin consisted of fluoridated carbona-
toapatite. The presence of this sparinglysoluble mineral at the
interface between the tooth and the restoration may providecaries resistance[188]. It wasdiscussed that theamount of flu-
oride released fromrestoratives and incorporated into enamel
is less important in lesion formation than the amount of flu-
oride released into the gap [66]. Extrapolation from in vitro
and in situ data indicated that a gap fluoride concentration
between 5 and 80 ppm might be the optimal range to prevent
caries formation [66,189]. Depending on the storage media,
both conventional and resin-modified glass-ionomers were
able to release fluoride in the required range (up to 100 ppm in
between 24 and 48 h after immersion). However, in the pres-
enceof a standardized interfacial gap,no preventive effect was
exerted in vivo from a glass-ionomer to protect the adjacent
enamel wall with respect to development of secondary caries[190].
With regard to fluoride released by restoratives which
are applied in a cavity it should be noted that acid etching
of dentin as performed in the total etching technique may
increase its permeability [191], and therefore also the depth
of fluoride uptake. Thereby, the preparation of self-etching
adhesives with pre-reacted glass-ionomer fillers increased
the release of fluoride from these experimental adhesives
[192]. Additionally, the application of hydrophilic primers may
improve the wetting of dentin andtherefore facilitate the pas-
sage of fluoride. In contrast, the hybrid layer formed after pre-
treatment of a cavity with an adhesive agent may reduce fluo-
ride diffusion. It shouldbe noted that a thick hybrid layer itselfmight act as acid-resistant layer hampering caries formation
[193]. These aspects should be taken into consideration when
anticaries activity of modern restoratives is estimated.
By summarizing these data, fluoride uptake of the adja-
cent dental hard tissueis higher in dentin andcementum than
in enamel, but is highly influenced by the interface between
restoration andtooth. Thereby, an intermediarymateriallayer,
such as an adhesivehybrid layer, may hamper fluoride uptake.
However, the amount of fluoride incorporated in dental hard
tissuesmight be of minor importance comparedto the fluoride
concentration in a fluid-filled microgap between the restora-
tionand the toothstructure. Thereby, severalrestorative mate-
rials might increase the fluoride concentration in the gap tothe required range between 5 and 80 ppm, which is estimated
to prevent caries.
8. Influence of fluoride-releasingrestoratives on caries development andprogression
8.1. Influence on demineralization of enamel adjacent
to fluoride-releasing restoratives
8.1.1. In vitro studies
In vitro, several fluoride-releasing restoratives have shown
to inhibit enamel and dentin demineralization produced by
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acidic gels or demineralizing buffer solutions. Thereby, inhi-
bition of enamel demineralization is located up to a distance
of 7 mm from the edge of the material (remote effect). When
compared with non-fluoride-releasing restorations, the place-
ment of glass-ionomers reduces mineral loss by almost 80%
at 0.22 mm distance from the restoration and by 37% 7 mm
distant from the restoration margin [194]. Glasspoole et al.
[195] examined the reductionin enamel demineralization pro-vided by fluoride-releasing glass-ionomers and composites.
Lesion areas were measured by polarized light microscopy
at distances from 100 to 800 m. At all distances, a signifi-
cant inhibition of enamel demineralization was seen for all
materials. Thereby, the degree of protection was highest in
the closest vicinity of the material, but lesion areas increased
with distance in an inverse relationship to the amount of
fluoride release [195]. These results were confirmed by micro-
radiographic assessment of artificial caries lesion depth and
mineral density of enamel adjacent to a conventional and a
resin-modified glass-ionomer. Forboth materials, lesion depth
increased and mineral density decreased with increasing dis-
tance (13 mm) from the restoration margin [196].As seen by polarized light microscopy, the placement of
conventional glass-ionomers results in a reduction of wall
lesion frequency and size of caries-like lesions in vitro. Reduc-
tion of enamel outer lesion size and depth ranged from 58 to
80% compared to the lesion size adjacent to non-fluoridated
filling materials [180,197199]. Wall lesion size and depth
were also decreased and amounted to approximately 30%
compared to the lesions adjacent to a non-fluoride-releasing
restorative [198]. For primary enamel samples it was shown
that placement of an amalgam-bonding resin with fluoride-
releasing capabilities provided a reduction of surface lesion
depth by 30% and a decrease in cavity wall lesion frequency
by 35% comparedto a conventionalamalgam restoration [200].Six to 10 weeks after insertion of different fluoride-
releasing materials, comparison of enamel surface and wall
lesion development and progression adjacent to the restora-
tion mostly revealed highest demineralization protection for
glass-ionomers (reduction of lesion size compared to non-
fluoridated control: 5880%), followed by resin-modified glass-
ionomers and compomers (reduction of lesion size compared
to non-fluoridated control: 3575%) and composites (reduc-
tion of lesion size comparedto non-fluoridated control: 940%)
[180,197199,201204].
The amount of fluoride in the restorative material seems
to influence the anticaries properties. In this sense, experi-
mental fluoride-releasing composites showed that wall lesiondevelopment and length of penetration of enamel deminer-
alization were more decreased adjacent to a resin containing
33% fluoride than for the composite containing 17% fluoride.
However, both experimental materials exhibited significantly
less demineralization of enamel surrounding the restoration
than a non-fluoridated composite and less or equal deminer-
alization than a fluoride-releasing silicate cement [205].
Other studies examined the remineralizing properties of
fluoride-releasing restoratives. The mean size reduction of
an artificial lesion adjacent to a fluoride-releasing composite
restoration amounted to 1227% after two weeks and 4080%
after three months compared to a non-fluoride-releasing
restorative [203].
8.1.2. In situ and in vivo studies
As shown in the above mentioned reports and investigations,
several in vitro studies found fluoride-releasing materials
effective in prevention of secondary caries. However, clinical
relevance of these artificial caries experiments is debatable.
Papagiannoulis et al. [190] evaluated the anticariogenicbehav-
ior of glass-ionomers and resin composite restorative materi-
als and found no correlation between in vivo andin vitro data.In vitro, glass-ionomer and fluoride-free composite restora-
tions applied in enamel cavities were stored in acidic gel for
four weeks to produce artificial caries-like lesions. For the in
vivo experiment, glass-ionomer and fluoride-free composite
restorations were inserted into premolars in a split-mouth
design. The premolars were extracted for orthodontic reasons
after six months. At regions without gaps, glass-ionomers
showed reduced lesion dimensions in vitro and no lesions
in vivo. At regions with gaps, no differences were found in
lesion depth between the tested materials in vitro, while in
vivo lesion dimensions were significantly greater for glass-
ionomers than for fluoride-free composites [190].
Currently, only few studies determined the demineraliza-tion behavior of enamel adjacent to fluoride-releasing restora-
tives in situ or in vivo [151,206209].
Kielbassa et al. [206,207] evaluated the effects of a con-
ventional and a resin-based glass-ionomer, different polyacid-
modified composites, an ion-releasing material and a compos-
ite on enamel lesion formationin situ. Thereby, intraoral appli-
ances were wornfor fourweeks without additional application
of topical fluorides. Only the ion-releasing material Ariston
leads to significantly lower lesion depth and mineral loss in
those areas of the developed caries lesions which were close
to the restoration. All other materials exhibited no preventive
effect on secondary caries formation [206,207].
As evaluated by microhardness measurement at variousdepths (10110m) and distances (130 and 230m) from
the edge of metallic restorations, fluoride-releasing resin-
modified or resin-based luting materials were not effective
in prevention of secondary caries of enamel and dentin in
situ [152]. In contrast, a fluoride-releasing glass-ionomer lut-
ing cement was able to reduce secondary caries development
in dentin but not in enamel [210]. The in situ simulation of a
highcariogenic challenge provoked significantlyhigher micro-
hardness values adjacent to a glass-ionomer cement than to
a non-fluoridated composite [151].
In a further in situ investigation, the effect of different
fluoride-containing composites (026 vol%fluoride)on enamel
demineralization around an artificial gap of 200m width was
quantified by micrographic measurements after one month.
At the gap margins,all fluoridated composites reducedenamel
demineralization (both lesion depth and mineral loss) signifi-
cantly with respect to the non-fluoridated control. At the outer
enamel surface next to the artificial gap, a beneficial effect of
fluoridation wasonly observed near to thecomposite with the
highest fluoride content [189]. It is noteworthy to mention that
fluoride concentration of the highly fluoridated experimental
composite was much higher than the content in commercially
available composites.
In conclusion, several in vitro studies found evidence for
an inhibition of enamel demineralization, while in situ and in
vivo studies found contradictory results, which do not allow
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for a final appraisal of the caries-inhibiting effects of fluoride-
releasing restoratives.
8.2. Influence on demineralization of dentin adjacent
to fluoride-releasing restoratives
8.2.1. In vitro studies
Several laboratory tests also investigated the ability of flu-oridated materials to prevent or inhibit demineralization of
adjacent dentin [180,211219].
Both conventional and resin-modified glass-ionomers as
well as compomers increased dentin resistance to cariogenic
or acidic challenges. Thereby, caries-like lesions in dentin
and cementum root surfaces adjacent to class V restora-
tions were reducedby 5463% (glass-ionomers), 2053% (resin-
modified glass-ionomers) or 1435% (compomers and giomer),
respectively, compared to non-fluoridated control materials
[211,212,217,220,221]. Also, fluoridated composites and amal-
gams reduced the depth of caries-like lesions adjacent to
restorations to 81 or 90.5%, respectively, compared to non-
fluoridated amalgams [217]. However, after immersion of rootdentin samples in a buffered demineralizing solution, an inhi-
bition zone adjacent to both conventional and resin-modified
glass-ionomer cements could be found which was less
frequently observed around a fluoride-releasing composite
[204].
Fluoride-releasing restoratives are also effective in preven-
tion of artificially created dentin wall lesions [180,212]. Size
of wall lesions adjacent to conventional or resin-modified
glass-ionomers was inhibited by 3040% compared to lesion
size adjacent to a non-fluoridated composite [180]. When
compared to unaltered materials, the incorporation of casein
phosphopeptideamorphous calcium phosphate or bioactive
glass into a glass-ionomer cement was associated with anincrease of fluoride release and an enhanced protection of the
adjacent dentin during acid challenge [27,28]. Also, the extent
of the cariostatic effect on root dentin provided by fluoride-
containing restoratives was evaluated by Knoop microhard-
ness measurement. While a fluoride-releasing composite and
a compomer exhibited no cariostatic effect, the extent of the
cariostatic effect was located up to 300m for the conven-
tional glass-ionomer and 150m for the resin-modified glass-
ionomer cement [222].
However, demineralization behavior at margins of fluoride-
releasing restorations might be influenced by topical fluo-
ride regimes. Glass-ionomers demonstrated significantly less
dentin demineralization than amalgam restorations when noexternal fluoride was applied or when the restorations were
either brushed with a fluoridated dentifrice twicedaily or were
exposed to a fluoride rinse. There was no significant difference
in dentin demineralization adjacent to the materials when
both a fluoride rinse and a fluoridated dentifrice were used
on a daily basis over 30 days [223].
Determination of lesion depth by confocal laser scan-
ning microscopy revealed differences in the caries-preventive
properties of fluoridated materials when used in chemical
or antimicrobial in vitro caries models [213]. Glass-ionomer
cement demonstrated anticarious properties for adjacent
dentin when exposed to a demineralizing solution (chemical
caries model). However, this was not true for glass-ionomer
and resin-modified glass-ionomer nor compomer and com-
posite restorations in a microbial caries model (inoculation
of the specimens to a solution containingStreptococcus mutans
and Lactobacillus casei) [213]. This findingwas confirmed in situ
when evaluating the remineralization of artificially deminer-
alized dentin beneath glass-ionomers, whendentin waseither
contaminated with bacteria or not [224]. One year after inser-
tion, nanohardness values of the bacteria-contaminated teethwere not different comparedto the nanohardness values three
days after insertion, but were significantly lower than in the
non-bacteria-contaminated dentin [224].
8.2.2. In situ studies
Currently, there is only one study available evaluating the
effects of fluoridated restoratives to dentin caries develop-
ment in situ [225]. Superficial caries-like lesions (25m depth
of demineralization) were submittedto severe plaque environ-
ment for three months in situ. Insertion of a glass-ionomer
restoration adjacent to the artificial demineralization zone
leads to a hypermineralization to an average depth of 125m.
Also, for deeper lesions (100 m) a hypermineralization of thedentin tissue up to a depth of 300 m could be observed. How-
ever, non-fluoridated amalgam or composite controls exhib-
ited either further demineralization or showed a large vari-
ety in the degree of demineralization or remineralization,
respectively. From these results the authors also concluded
that hypermineralization as promoted by the glass-ionomer
cement may increase the acid resistance by limiting the num-
ber of diffusion pathways for acids formed in plaque [225].
Even though in vitro studies found evidence for the caries-
inhibiting effect of fluoride-releasing restoratives on dentin,
the small amount of in situ data do not suffice for final con-
clusions.
8.3. Clinical studies evaluating secondary caries
adjacent to fluoride-releasing restoratives
Despite the cariostatic effects possibly achieved fromfluoride-
releasing materials, secondary caries is still one of the main
reasons for clinical failure of restorations (for review see
[226228]).
Unfortunately, only fewlongitudinal studies with an obser-
vation period of three and more years exist which evalu-
ate secondary caries adjacent to fluoride-releasing and non-
fluoride-releasing materials. To estimate the impact of flu-
oride release on secondary caries development, split-mouth
designed studies evaluating different materials in the samepatients seem to be more appropriate than studies dealing
with a single material in the respective patients. In split-
mouth designed studies, test and control material are sub-
jected to the same individual conditions and caries risk
parameters. With regard to secondary caries development,
however, these studies showed contradictory results.
Three-year success rate of class II restorations performed
with either a compomer (Compoglass) and a non-fluoridated
composite (TPH-Spectrum) [229] or a compomer (Dyract) and
a non-fluoridated amalgam (Tytin) [230] found no differences
between the materialsin relation to caries development in pri-
mary molars. Also, a three-year clinical evaluation of either a
compomer (Dyract), a composite (TPH-Spectrum) and a com-
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pomer/composite (sandwich-technique, Dyract layered with
TPH-Spectrum) [231] or a compomer/composite sandwich
restoration anda composite restoration [232] of class II cavities
found no differences in secondary caries development. These
results are also confirmed for class I compomer/composite
(sandwich) and composite restorations during an observation
period of six years [233].
Van Dijken [234] found no differences in secondarycaries development of class III cavities restored with a
polyacid-modified glass-ionomer (Dyract), a conventional
glass-ionomer (Fuji II LC) and a composite (Pekafill) in a three-
year observation period. Also, an intra-individually compari-
son of ceramic inlays luted with either a resin-modified glass-
ionomer cement (Fuji Plus) or a resin composite (Panavia)
revealed no significant differences in secondary caries in a
five-year clinical evaluation [235].
In contrast, clinical evaluation of paired compomer(Dyract)
and glass-ionomer (Chemfil Superior) classes I and II restora-
tions in primary molars revealed significantly better perfor-
mance with regard to caries development for Dyract than
for Chemfil Superior. Fifteen restorations failed during thefollow-up period of 42 months. Thereby, six glass-ionomer
restorationsbut none of the compomer restorations failed due
to recurrent caries [236]. Also, comparison of conventional
(Fuji II) and resin-modified glass-ionomer (Vitremer) class II
restorationsof primary molars exhibitedless secondary caries
at the margins of the resin-modified glass-ionomer (none of
53 restorations) than at themargins of the conventional glass-
ionomer (4 of 62 restorations) [237]. Three-year examination
of resin-modified glass-ionomer and amalgam class II restora-
tions of primary molars exhibitedalso better caries-preventive
properties for the resin-modified glass-ionomer. While clin-
ical evaluation found no differences between the materials,
polarizedlight microscopy of the exfoliated teeth revealed sig-nificantly lessenamel demineralization at restoration margins
of the resin-modified glass-ionomer than at the margins of
the amalgam restoration [238]. Six-year follow-up assessment
of class I restorations in permanent molars exhibited signif-
icantly more secondary caries for amalgam (10%) compared
to glass-ionomers (2%) [239]. In another five-year evaluation
of glass-ionomer (Ketac-Fil) and amalgam (Amalcap) restora-
tions in deciduous molars, the glass-ionomer had a lower
survival time and showed greater loss of anatomic form and
marginal integrity, but less recurrent caries compared to the
amalgam [240]. However, fluoridated amalgam used in class
I cavities of permanent molars exhibited less caries develop-
mentwithin fouryears comparedto non-fluoridated amalgam[241].
9. Influence on caries formation of teethlocated in interproximal contact tofluoride-releasing restoratives
9.1. In vitro and in situ studies
It is also discussed whether fluoride-releasing restoratives
might be effective in inhibition of incipient carious lesions
of neighboring teeth located in interproximal contact to the
restoration.
In vitro andin situ investigations found that glass-ionomer
and resin-modified glass-ionomer restorations in direct con-
tact to adjacent teeth prevent demineralization compared to
non-fluoridated amalgam and composite [209,242]. However,
additional application of topical fluoride (fluoridated denti-
frice) significantly increased remineralization and decreased
demineralization,respectively, in all groups independent from
the material [209,242]. This was also confirmed in anotherin situ investigation, where glass-ionomers showed some
slight caries-preventive effects compared to a fluoridated and
a non-fluoridated composite when subjects performed oral
hygiene without topical fluorides. The regular application of
fluoridated toothpaste was, however, effective in prevention
of secondary caries in all experimental groups [243]. In vitro,
it could also be shown that placement of a resin-modified
glass-ionomer exhibited nearly the same remineralization
effects on adjacent caries as toothpaste application twice
daily, but both fluoride regimes were less effective than the
daily use of a fluoridated rinse [244]. A one-year evaluation
of glass-ionomer, resin-modified glass-ionomer and resin
composite class V restoration in xerostomic head and neckradiation patients found differences depending on the fre-
quency of topical fluoridation. No recurrent caries was found
in patients using fluoride gels at regular intervals. However, in
patients using fluoride gels at irregular intervals, less enamel
caries was evident for glass-ionomer and resin-modified
glass-ionomer restorations than for composite fillings
[245].
Therefore, it is assumed that topical fluoridation over-
whelmingly increases the ability of the fluoridated restora-
tives to inhibit demineralization and promote remineraliza-
tion on the adjacent interproximal incipient caries lesion. On
the other hand, it might be postulated that theuse of fluoride-
releasing restoratives does provide additional protection forpatients who might not strictly follow the recommended pro-
phylactic measures.
The effect of a glass-ionomer, a resin-modified glass-
ionomer, a compomer and a non-fluoridated composite on
sound enamel of approximal teeth without additional topical
fluoride treatment was also evaluated in situ. Specimens were
worn for 70 days under cariogenic conditions. Enamel micro-
hardness assessment was located at 0, 0.4, 0.8 and 1.2mm
distances from the contact point. Microhardness alteration
wasgenerally lowest for the resin-modified glass-ionomer, fol-
lowed by the conventional glass-ionomer and the compomer.
The resin-modified glass-ionomer exhibited none and glass-
ionomers and compomers only slight alterations, while thenon-fluoridated composite showed distinct formation of sub-
surface enamel lesions [208]. Also, remineralization of artifi-
cial caries-like lesions adjacent interproximally to teeth with
class II restorations was higher in metal-reinforced glass-
ionomers and amalgam than in glass-ionomer/resin compos-
ite restorations [246].
9.2. Clinical studies
Currently, onlyfew clinical studiesexist concerning the effects
of fluoride-releasing restoratives at the caries development of
proximal tooth surfaces.
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d e n t a l m a t e r i a l s 2 3 ( 2 0 0 7 ) 343362 355
In a three-year study in split-mouth design, caries develop-
ment on tooth surfaces adjacent to class II amalgam (Disper-
salloy) and glass-ionomer tunnel restorations was assessed.
While the materials exhibited no differences with regard to
secondary caries development at the restoration margins, pri-
mary caries was significantly reduced on tooth surfaces adja-
cent to the glass-ionomer restorations as compared to sur-
faces in contact to amalgam restorations [247]. A seven-yearstudy on three resin-modified glass-ionomer cements (Fuji II
LC, Photac-Fil and Vitremer) and a compomer (Dyract) showed
that the restorative material and cavity conditioning influ-
enced the survival of the restoration but not the progression
of caries on adjacent surfaces [248].
In summary, clinical studies exhibited inconsistent results
concerning the prevention of secondary caries by fluoride-
releasing restoratives. Despite the high release of fluoride ions
in some studies, secondary caries has been found to be the
main reason for the clinical failure of glass-ionomer restora-
tions [249,250]. Furthermore, glass-ionomer cements are not
considered as having adequate mechanical strength for gen-
eral use as definitive restorations in stress-bearing posteriorteeth (for review see [251]). Thereby, the annual failure rate
of glass-ionomers (7.2%) is distinctly higher as compared to
direct composite (2.2%), compomer (1.1%) or amalgam (3.0%)
restorations [251]. In contrast to glass-ionomers, compomer
and composite restorations exhibit a good clinical perfor-
mance over time concerning marginal integrity and discol-
oration, surface texture, anatomic form and occlusal wear.
However, although compomers and some composites are able
to release fluoride in a range that might have cariostatic effi-
cacy, it is still unproven whether their good clinical perfor-
mance is attributed to their ability to release fluoride. There-
fore, further investigations are necessary to determine the
impact of fluoride-releasing compomer and composite mate-rials on secondary caries formation. Furthermore, the devel-
opment of restorative materials with excellent mechanical
properties and a constant release of high amounts of fluoride
seem recommendable.
10. Conclusion
There is a continuum of restorative materials that range from
initially high fluoride release (conventional glass-ionomer
and resin-modified glass-ionomer) to intermediate fluoride
release (compomer) to low fluoride release (fluoride-releasing
composite and fluoride-releasing amalgam) to no fluoriderelease (non-fluoridated composite resins and amalgam)
[10,11,15,55,59,252,253]. However, the potential to release flu-
oride not only varies between different restorative materi-
als, but also within different brands. Optimal fluoride release
(short- and long-term release) from a restorative is related to
their matrices, setting mechanisms and fluoride content and
depends on several environmental conditions. Thereby, flu-
oride release is substantial only in the period immediately
following placement of the fresh material. However, it is not
evident whether initial burst or long-term release may be
clinically more important to prevent caries as certain rem-
ineralizing mechanisms need rather low but constantly pro-
vided quantities of fluoride. Nevertheless, fluoride-releasing
materials may act as a reservoir for fluorides from topical flu-
oridation and may lead to an elevation of the fluoride level
in plaque or saliva in the immediate vicinity of the restora-
tive. Despite the cariostatic effects achieved from an increase
of fluoride content in saliva, plaque and dental hard tissues,
clinical studies exhibited conflicting data as to whether or not
these materialssufficientlyprevent or inhibit secondary caries
compared to non-fluoridated restoratives. Therefore, furtherclinical studies, preferably in split-mouth design, are needed
to evaluate the impact of fluoride-releasing restoratives on
secondary caries development and progression especially in
patient groups that have limited access to or low compliance
with prophylactic measures.
Acknowledgement
The study was supported by a grant of the DENTSPLY DeTrey
GmbH.
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